The characteristics of polyvinylpyrrolidone (PVP)-stabilised nano-zero-valent iron (PVP-NZVI) and its application, combined with surfactant, to trichloroethylene (TCE)-contaminated soil were investigated. Two surfactants (cetyltrimethylammonium bromide [CTAB] and sodium dodecyl sulphate [SDS]) were tested for their ability to enhance the remedial activity of PVP-NZVI in 3 h batch experiments. The prepared PVP-NZVI formed nanoparticles ∼70 nm in diameter. The isoelectric point of PVP-NZVI was about 8.51, similar to the initial pH. X-ray diffraction and X-ray photoelectron spectroscopy analyses revealed that ZVI was the main active component of PVP-NZVI, and carbonised products of the target were observed. The TCE dechlorination efficiency by PVP-NZVI was about 84.73%; the efficiency by PVP-NZVI was about 20% higher when combined with SDS than with CTAB. Therefore, application of PVP-NZVI with SDS represents a potential remediation approach for TCE-contaminated soil.